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arXiv:1805.09482v1 [physics.atom-ph] 24 May 2018

Experimental and Theoretical Investigation of the Crossover from the Ultracold to the Quasiclassical Regime of Photodissociation

I. Majewska, 1 S. S. Kondov, 2 C.-H. Lee, 2 M. McDonald, 2, B. H. McGuyer, 2, R. Moszynski, 1 and T. Zelevinsky 2,

1 Quantum Chemistry Laboratory, Department of Chemistry, University of Warsaw, Pasteura 1, 02-093 Warsaw, Poland 2 Department of Physics, Columbia University, 538 West 120th Street, New York, NY 10027-5255, USA

At ultralow energies, atoms and molecules undergo collisions and reactions that are best described in terms of quantum mechanical wave functions. In contrast, at higher energies these processes can be understood quasiclassically. Here, we investigate the crossover from the quantum mechanical to the quasiclassical regime both experimentally and theoretically for photodissociation of ultracold diatomic strontium molecules. This basic reaction is carried out with a full control of quantum states for the molecules and their photofragments. The photofragment angular distributions are imaged, and calculated using a quantum mechanical model as well as the WKB and a semiclassical approximation that are explicitly compared across a range of photofragment energies. The reaction process is shown to converge to its high-energy (axial recoil) limit when the energy exceeds the height of any reaction barriers. This phenomenon is quantitatively investigated for two-channel photodissociation using intuitive parameters for the channel amplitude and phase. While the axial recoil limit is generally found to be well described by a commonly used quasiclassical model, we find that when the photofragments are identical particles, their bosonic or fermionic quantum statistics can cause this model to fail, requiring a quantum mechanical treatment even at high energies.

I.

INTRODUCTION

Low-temperature atomic and molecular collisions and reactions are qualitatively different from their high- energy counterparts. While the latter can usually be explained quasiclassically, the former are strongly in- fluenced by the wave nature of the particles and are correctly described only with quantum mechanical wave functions. In addition, at very low temperatures, precise control of internal molecular states is possible, permit- ting studies of state-specific reaction cross sections rather than statistical averages. Ultracold, quantum mechanical chemistry has many distinguishing features such as reac- tion barrier tunneling, quantum interference, and possi- bilities for controlling the outcome with applied electric or magnetic fields [1]. On the other hand, a quasiclassical interpretation can offer intuitive insight into complicated processes. In particular, photodissociation [2–4] has been exten- sively used to study the nature of molecular bonding, which becomes encoded in angular distributions of the outgoing photofragments. It is one of the most basic chemical processes, and is highly amenable to quantum state control of the outgoing particles, since the reaction proceeds without a collision. The majority of photodis- sociation experiments to date have been carried out in a regime that is well described in the quasiclassical frame- work [5–8], while recently we studied this reaction in the purely quantum regime to observe matter-wave interfer-

Present address: Department of Physics, University of Chicago, 929 East 57th Street GCIS ESB11, Chicago, IL 60637, USA Present address: Facebook, Inc., 1 Hacker Way, Menlo Park, CA 94025, USA tanya.zelevinsky@columbia.edu

ence of the photodissociation products [9] and control of the reaction by weak magnetic fields [10]. In this work, we show that the photodissociation energy can be tuned by several orders of magnitude to span the range from the quantum mechanical to the quasiclassical regime. Ex- perimentally and theoretically we demonstrate how the crossover occurs and what determines its energy scale. We also find that if the photofragments are identical bosonic or fermionic particles, then the reaction outcome is not always well described in quasiclassical terms even at high energies and the effects of quantum statistics can persist indefinitely. Moreover, we apply the Wentzel- Kramers-Brillouin (WKB) approximation to photodisso- ciation, as well as a related semiclassical approximation, and discuss how accurately they capture the transition from ultracold to quasiclassical behavior.

In the experiment, we trap diatomic strontium molecules ( 88 Sr 2 ) at a temperature of a few microkelvin, enabling precise manipulation and preparation of specific quantum states as the starting point for photodissocia- tion. The photodissociation laser light has strictly con- trolled frequency and polarization, yielding photofrag- ments in fully defined quantum states. The ab initio theory is aided by a state-of-the-art molecular model [11, 12] that captures the effects of nonadiabatic mixing and yields excellent agreement with spectroscopic mea- surements [13–16].

This approach offers a unique opportunity to finely scan a large range of energies that is relevant to the crossover from distinctly quantum mechanical to quasi- classical photodissociation. Since initial molecular states have low angular momenta, the relevant dynamics occurs at very low, millikelvin energies. The experiment can sample energies from 0.1 mK limited by the molecule trap depth to 100 mK limited by the available laser in- tensity that is needed to overcome the diminishing tran-

2

sition strengths. The rotational and electronic potential barriers that are explored in this and related [17] work fall within this range, permitting direct observations of the crossover. We reduce the process to a single initial molec- ular state and two angular-momentum product channels, in which case the quantum mechanics of the reaction can be encoded in a single pair of coefficients: the amplitude and phase of the channel interference. Note that in both quantum and quasiclassical regimes we work with single initial quantum states. The classical nature of the process emerges not because of statistical averages over the initial states, but when the kinetic en- ergies of the photofragments are large. At high energies, the photodissociation time scale is much faster than the time scale of molecular rotations, and the molecules can be described as classical rotors. An equivalent view is that the photodissociation outcome should have quasi- classical behavior if the photofragment energy in the con- tinuum exceeds the height of any potential barriers. This regime is referred to as axial recoil, where the molecule has insufficient time to rotate during photodissociation and the photofragments emerge along the instantaneous direction of the bond axis. Here we investigate at what energies the axial recoil regime is reached, whether it is accurately described by a quasiclassical model, and how its onset depends on the molecular binding energy and angular momentum. In Sec. II of this work, we describe the photodissoci- ation experiment and show the measured and calculated photofragment angular distributions. In Sec. III, we discuss the quantum mechanical photodissociation cross section used in calculating the angular distributions, its axial recoil limit, and the quasiclassical model. Section IV details the crossover from the ultracold to the quasi- classical regime for a range of molecular binding energies and angular momenta and shows the onset of the axial recoil limit at energies that exceed the potential barriers in the continuum. In Sec. V we discuss the breakdown of the quasiclassical picture of photodissociation in case of identical photofragments and present the correct high- energy limit that takes quantum statistics into account. We summarize our conclusions in Sec. VI.

II.

THE PHOTODISSOCIATION EXPERIMENT

The starting point for the experiment is creation of 7, 000 weakly bound ultracold 88 Sr 2 molecules in the electronic ground state. This is accomplished by laser cooling, trapping, and photoassociating Sr atoms in a far-off-resonant optical lattice [18]. Subsequently, optical selection rules allow specific molecular quantum states to be populated and serve as a starting point for photodis- sociation. Figure 1 shows the photodissociation experiment from the point of view of molecular potentials and wave func-

tions. The ground state gerade potential X0

+

g

correlates

to the 1 S + 1 S atomic threshold, while the singly-excited

J = 0 J = 2 V (R )
J = 0
J = 2
V (R )

R

FIG. 1. Molecular potentials for the 88 Sr 2 electronic states

used in this work. The ground state X0

g

+

correlates to the

+

and

u

1 S + 1 S atomic threshold while the excited states 0

1 u correlate to 1 S + 3 P 1 . The 1 u potential has a 1 mK

electronic barrier. The molecules are photodissociated via an

electric-dipole optical transition from bound states of mostly

0

+

u

or 1 u character to the ground-state continuum. A range

of rovibrational initial states are explored. In this example,

weakly bound 0

+

u

(v = 2, J i = 1, M i = 0) molecules are

photodissociated, and the photofragments occupy two allowed partial waves J = {0, 2} shown at the energy of 50 MHz (2.4 mK).

ungerade potentials 0

+

u

and

1 u

correlate to

1 S + 3 P 1 ,

where the 0 and 1 state labels correspond to Ω, the pro-

jection of the total atomic angular momentum onto the molecular axis. Weakly bound ground-state molecules

are excited to 0

+

u

and 1 u bound states with a laser pulse,

and the resulting molecules are immediately photodisso- ciated to the ground-state continuum. The bound states are labeled by their vibrational quantum number v (neg- ative numbers count down from the threshold), total an- gular momentum J, and its projection M onto the quan-

tization axis that is set by a small vertical magnetic field.

In Fig. 1, the 0

+

u

(v = 2, J i = 1, M i = 0) molecules are

photodissociated by 689 nm light. The allowed angular- momentum states, or partial waves, in the continuum are J = {0, 2} due to electric-dipole selection rules as well as the bosonic nature of 88 Sr that allows only even J values in the ground state.

The photodissociation laser light co-propagates with the lattice laser and both are focused to a 30 µm waist at the molecular cloud. A broad imaging beam, resonant with a strong 461 nm transition in atomic Sr, nearly co- propagates with the lattice and is directed at a charge- coupled device camera that collects absorption images of the photofragments. A typical experiment uses 10 µs long photodissociation laser pulses, 100 µs of free expansion, and 10 µs absorption imaging pulses [17]. Several hundred images are averaged in each experiment.

The experimental and theoretical results of photodis- sociating the molecules in a range of precisely prepared quantum states are shown in Fig. 2. In this set of measurements, light polarization is along the quan-

3

(a)

(b)

ε/h= 13 MHz 33 53 100 300 WKB 0 u + (-5,1,0) 0 u + (-4,1,0)
ε/h= 13 MHz
33
53
100
300
WKB
0 u + (-5,1,0)
0 u + (-4,1,0)
0 u + (-3,1,0)
0 u + (-2,1,0)
13 33 53 100 300 1 0 (c) 0 quantum u + (-2,1,0) WKB 0 u
13
33
53
100
300
1
0
(c)
0
quantum u + (-2,1,0)
WKB 0 u
Axial limit recoil
+
Srdensity (norm.)
WKB
1 u (-2,1,0)
1 u (-1,1,0)
1000 MHz
1000 MHz

1000 MHz

3 (a) (b) ε/h= 13 MHz 33 53 100 300 WKB 0 u + (-5,1,0) 0

quantum u (-2,1,0)

1

WKB 1 u

Axial limit recoil

1000 MHz

1000 MHz

3 (a) (b) ε/h= 13 MHz 33 53 100 300 WKB 0 u + (-5,1,0) 0

FIG. 2. Measured and calculated photofragment angular distributions in the ultracold quantum mechanical regime and in the

high-energy axial recoil limit. (a) The 0

+

u

initial states are explored at the continuum energies ε/h = {13, 33, 53, 100, 300}

MHz (ε/k B =0.6-14 mK). For each initial state, the top and bottom rows correspond to measurements and quantum mechan- ical theory, respectively. The ab initio images were adjusted for the shell size and thickness in experimental data, where the photofragment ring diameter is typically 0.3-0.5 mm. The strong dependence of the patterns on ε and the less pronounced dependence on v are discussed in the text. The lowest row shows v-independent distributions obtained with the WKB approx- imation. The most weakly bound state exhibits central dots that arise from spontaneous photodissociation into the optical

lattice; these are more apparent at higher energies where the signal is weaker, and can be ignored. (b) Same as (a), for 1 u

initial molecular states. (c) Angular distributions calculated for a pair of 0

+

u

and 1 u weakly bound states using both quantum

theory and the WKB approximation at a high energy ε/h = 1000 MHz (ε/k B = 48 mK), to show their close agreement with

the appropriate axial recoil limit.

tization axis and the molecules start from J i = 1,

M i

=

0.

In Fig.

2(a), molecules in vibrational states

  • v = {−2, 3, 4, 5} of 0

+

u

are photodissociated. The

photofragment angular distributions show a strong en-

ergy dependence, and a less pronounced dependence on

  • v except for the most weakly bound levels, as discussed

in Sec. IV A. The bottom row of theoretical images is

obtained with the WKB approximation, which is inde-

pendent of v and described in Sec. IV B. Figure 2(b) is analogous to (a) but illustrates 1 u initial states. A good agreement between measurements and quantum mechan- ical calculations is reached for all initial states and con- tinuum energies. Figure 2(c) shows agreement between quantum theory and the WKB approximation at the con- tinuum energy ε/h = 1000 MHz (ε/k B = 48 mK) where h = 2π and k B are the Planck and Boltzmann con-

4

stants. At this high energy, both methods approach the

axial recoil limit which is also shown.

  • A. General quantum mechanical model

The general quantum mechanical expression for the

photodissociation cross section is based on Fermi’s golden

rule with the electric-dipole (E1) transition operator,

σ QM (θ, φ)

Ψ
Ψ

JM

k

({r}, R) T

E1

ˆ

1

Ψ J i M i i ({r}, R) ,

2

(1)

III.

PHOTOFRAGMENT ANGULAR DISTRIBUTIONS

Sections III A-III E overview the quantum mechanical

calculation and parametrization of the photodissociation

cross section both in the low-energy regime and in the

high-energy axial recoil limit, as well as the correspon-

dence of the latter to the quasiclassical approximation.

where {r} is the set of atomic electronic coordinates, R

is the vector connecting the photofragments, k is the lab-

frame wave vector of the photofragments, Ψ

JM

k

is the fi-

nal (continuum) wave function, and Ψ J i M i i is the initial

(bound) wave function. The polar and azimuthal angles

{θ, φ} are referenced to the quantization axis.

Assuming a pure initial state |J i M i i , expanding the

bound and continuum wavefunctions into the products

of their electronic, rovibrational and angular parts, in-

tegrating over the rotation angles and summing over M

transforms Eq. (1) into

σ QM (θ, φ) ∝ (−1) M k +Ω k (2J k + Ω k J
σ QM (θ, φ) ∝
(−1) M k +Ω k (2J k +
Ω k
J k (M k )P Qn k

1)D

J k

M

k k (φ, θ, 0)

(2)

×

J k

M k

1

P

M i k

J i

J k

1

Q

2 J i J k k Ω k (R) |d BF | χ n i J
2
J i
J
k
k Ω k (R) |d BF | χ n i J i Ω i (R) ,
n
i χ

where χ n (R) are the rovibrational wave functions in-

dexed by all the relativistic electronic channels that are

included in the model, d BF is the body-fixed E1 tran-

sition operator, J k are the indexed continuum angu-

J

lar momenta, D M are Wigner rotation matrices, and

Q = Ω k i (a photodissociation transition is called

parallel if Q = 0 and perpendicular if |Q| = 1). The

polarization index P = 0 or P = ±1 if the photodisso-

ciation light is polarized along or perpendicularly to the

quantization axis, respectively (such that P = M k M i ).

  • B. Axial recoil approximation

At low photofragment energies, to obtain the correct

photodissociation cross sections it is crucial to calculate

the matrix elements χ

J k

(R)|d BF |χ n i J i i (R) in Eq.

n k k

(2). At high energies, these matrix elements become in-

dependent of J k [7] and can be simply factored out of Eq.

(2). This is equivalent to disregarding the photodissoci-

ation dynamics. Under this axial recoil approximation,

the photodissociation cross section (2) reduces to

σ(θ, φ) AR ∝ (−1) M k +Ω k (2J k + 1)D Q J k
σ(θ, φ) AR ∝
(−1) M k +Ω k (2J k + 1)D
Q
J k P
2 J k 1 J i J k 1 J i J k k Ω k
2
J k
1
J i
J k
1
J i
J k
k Ω k (φ, θ, 0)
.
(3)
M
−M k
P
M i −Ω k
Q
i
  • C. Two-parameter quantum mechanical model

Consider

the

photodissociation

of

0

+

u

(v, J i , M i )

molecules to the ground-state continuum with P = 0.

For odd

menta in

J i

(which are the only allowed angular mo-

0

+

u

due to quantum statistics), the allowed

angular momenta in the continuum are J = J i 1 and

J i + 1, while M = M i . Then the quantum mechanical

photofragmentation cross section can be expressed using

only two parameters, the channel amplitude-squared R

5

and the relative channel phase δ:

σ Rδ (θ, φ)

(4)

RY J i 1,M i (θ, φ) + (1) i e iδ 1 RY J i +1,M i (θ, φ)

2

.

The (1) i factor correctly connects the sign of the δ

parameter to the phase shift between the continuum wave

5 and the relative channel phase δ : σ ( θ, φ ) ∝ (4) RY

functions, and Y JM are spherical harmonics which are

proportional to the angular wave functions for Ω = 0.

The expression for the R parameter can be derived by

comparing Eq. (4) to the traditional cross section (2).

We obtain

R =

2J i 1 J i 1

M k

1

P

M i J i 1

J i

0

1

i

i χ

J i

J=J i1

n k k

(R)

|d BF | χ n i J i i (R)

2

×

J k ={J i 1,J i +1}

2J k + 1

J k

M k

1

P

M i k

J i

J k

1

Q

i χ

J i

k k (R) |d BF | χ n i J i i (R)

J k

n

2

1

.

(5)

The δ parameter is calculated as the phase shift difference

for the continuum wave functions, δ = δ J i +1 δ J i 1 .

In the axial recoil limit Eq. (5) is simplified by setting

the matrix elements to a constant and canceling them, as

explained in Sec. III B. This results in values of R that

approach 0.5 with increasing J i , while the phase shifts

become identical: δ J i +1 δ J i 1 , yielding δ 0 and

cos δ 1.

  • D. Quasiclassical model

The

commonly

used

quasiclassical model for

photofragment angular distributions [5, 6] describes

the photodissociation cross section as

σ QC (θ, φ) P i (θ, φ) × [1 + β 2 P 2 (cos θ)] ,

(6)

J

where P i (θ, φ) = |D M i i (φ, θ, 0)| 2 is the probability den-

i

sity of the initial molecular orientation. The anisotropy

parameter is β 2 = 2 for parallel photodissociation tran-

sitions (Q = 0) and β 2 = 1 for perpendicular transi-

tions (|Q| = 1). If the molecule is in a superposition

of |J i M i i states, the initial probability density can be

generalized as [8]

P i (θ, φ) =

J i J M i M

i

i

i

J

D M i i (φ, θ, 0)D

i

i

M

i

i (φ, θ, 0).

J

(7)

Note that in Eq. (7) there are no cross terms for Ω i .

The intuition behind Eq. (6) is that the photofragment

angular distribution follows the initial angular density of

the molecule, modified by the angular probability density

of the photon absorption.

5 and the relative channel phase δ : σ ( θ, φ ) ∝ (4) RY
  • E. Correspondence of the quasiclassical model to the axial recoil approximation

It was shown in Ref. [7] that for photodissociation light

polarized along the quantization axis, Eq. (3) reduces to

J

σ AR (θ, φ) ∝ |D M i i | 2 × [1 + β 2 P 2 (cos θ)] for initial states

i

with a single Ω i [8]. We have confirmed that this re-

sult also holds for other polarizations of the photodisso-

ciating light (if the light polarization is perpendicular to

the quantization axis, P 2 (cos θ) should be replaced with

P 2 (sin θ sin φ)).

Therefore the quasiclassical model (6) can be applied

in the axial recoil limit to obtain angular distribution

predictions that are identical to those of the quantum

mechanical model. However, an important assumption in

Refs. [7, 8] is that the photofragments are not identical

quantum particles. Deviations from this assumption are

discussed in Sec. V.

IV.

CROSSOVER FROM THE ULTRACOLD

REGIME TO THE AXIAL RECOIL LIMIT

We investigate the crossover from the ultracold quan-

tum mechanical to the high-energy axial recoil regime

of photodissociation, as observed in Fig. 2. The intu-

itive parametrization of Eq. (4) that accurately illus-

trates two-channel photodissociation allows us to study

the crossover as it applies to only two parameters, R and

δ. These parameters can have a strong energy depen-

dence in the ultracold regime while approaching their

axial recoil values at higher energies. In this Section,

we address the following questions: at what energy scale

does the outcome of photodissociation approach the ax-

ial recoil limit; how does this energy scale depend on the

molecular binding energy (or vibrational level) and ro-

tational angular momentum; and how well do the WKB

and semiclassical approximations model this crossover?

6

(a)

 
v= -2 v= -3 v= -5 v= 0 v= -4
v= -2 v= -3 v= -5 v= 0 v= -4
v= -2
v= -3
v= -5
v= 0
v= -4
(a) v= -2 v= -3 v= -5 v= 0 v= -4 R ε / h (MHz)

R

 
(a) v= -2 v= -3 v= -5 v= 0 v= -4 R ε / h (MHz)
(a) v= -2 v= -3 v= -5 v= 0 v= -4 R ε / h (MHz)
(a) v= -2 v= -3 v= -5 v= 0 v= -4 R ε / h (MHz)
 
(a) v= -2 v= -3 v= -5 v= 0 v= -4 R ε / h (MHz)
(a) v= -2 v= -3 v= -5 v= 0 v= -4 R ε / h (MHz)
(a) v= -2 v= -3 v= -5 v= 0 v= -4 R ε / h (MHz)
(a) v= -2 v= -3 v= -5 v= 0 v= -4 R ε / h (MHz)
(a) v= -2 v= -3 v= -5 v= 0 v= -4 R ε / h (MHz)
 

ε/h (MHz)

(b)

V (r)

J = 0 J = 2
J = 0
J = 2

trated for the 0

+

u

(2, 1, 0) wave function in Fig. 1. The

continuum wave functions, as also shown in Fig. 1, are

similar at small internuclear separations but undergo a

relative phase shift at larger distances that correspond to

the bond length in initially very weakly bound molecules.

This can prevent photodissociation from reaching quasi-

classical behavior at the expected energies. The energy

dependences for v = 4, 5 (bound by 10 3 MHz) are

more regular, and we find that all the deeper vibrational

levels starting from v = 10 (bound by 10 5 MHz)

exhibit nearly identical behavior illustrated in Fig. 3(a)

by the deepest v = 0 level (bound by 10 8 MHz). We

conclude that with the exception of asymptotic molecules

that are bound just below threshold, the R parameter is

independent of the vibrational quantum number. Since

the δ parameter is v-independent as discussed in Sec.

IV B, the expected anisotropy patterns are nearly inde-

pendent of the binding energy, or v. We have checked

that for higher initial angular momenta J i , the R param-

eter is also independent of v except for the most weakly

bound molecules.

6 (a) v= -2 v= -3 v= -5 v= 0 v= -4 R ε / h

r (a 0 )

  • It is clear from Fig. 3(a) that R 1 as ε 0, indi-

cating that the lowest partial wave (J = 0 in this case)

dominates the photofragment distribution at ultralow en-

FIG. 3. (a) Quantum mechanical calculation of the amplitude-squared R parameter for two-channel photodisso-

ciation as in Eq. (4). The initial molecular state is 0

+

u

(v, 1, 0)

with v = {−2, 3, 4, 5}, and P =

0. For comparison, the

most deeply bound v = 0 state is also shown. The axial recoil limit is indicated with a dashed line. (b) The allowed con- tinuum wave functions with J = {0, 2} are plotted for very low energy ε/h = 0.5 MHz (ε/k B = 24 µK). The negligible contribution of the J = 2 partial wave due to its repulsive ro- tational barrier explains why R = 0 as ε 0 in (a) and thus only the lowest allowed partial wave is populated in near- threshold photodissociation.

ergies. This is caused by the suppression of low-energy

scattering wave functions with higher angular momenta

at relevant internuclear separations, due to their rota-

tional barriers. Figure 3(b) shows the J = 0 and J = 2

wave functions at the low continuum energy of ε/h = 0.5

MHz (ε/k B = 24 µK), where J = 2 is strongly suppressed

at the relevant molecular bond lengths of 100 bohr.

The crossover from the ultracold, quantum mechanical

regime to the axial recoil limit is explored in Fig. 4 as

a function of the initial angular momentum J i . The R

parameter is plotted as a function of energy for different

odd J i of initial states within the 0

+

u

and 1 u electronic

manifolds, assuming M i = P = 0. The calculations were

  • A. Approaching the axial recoil limit: Channel amplitude

The R parameter from Eq. (4) depends on both the

bound and continuum wave functions, as can be explicitly

seen from Eq. (5). Therefore, its behavior as a function

of continuum energy can depend on the vibrational state

of the molecule, potentially influencing the energy scale

at which the axial recoil limit is reached based on the

molecular binding energy. The plots in Fig. 3(a) show

the R parameter for several weakly bound initial states

+

  • 0 u

(v, J i = 1, M i = 0) with v = {−2, 3, 4, 5}

as well

as for the most deeply bound state v = 0. The dashed

performed for the most deeply bound vibrational level

v = 0 to avoid any dependence on v. For all initial states,

R = 1 at threshold and decays to the axial recoil limit

(shown with horizontal lines) as a function of energy. In

each frame, a vertical line marks the rotational barrier

height corresponding to the largest partial wave in the

continuum, J i + 1. As expected, the barrier height sets

the energy scale for the onset of the axial recoil regime.

This trend is evident despite the irregularities connected

to shape resonances for J = {4, 8, 20} (the J = 4 shape

resonance has been experimentally detected [9]).

line indicates the axial recoil limit.

For some of the shallow vibrational levels such as

  • B. Approaching the axial recoil limit: Channel phase and various approximations

v = 2, 3 (bound by 10 2 MHz) the R parameter

shows strong energy dependence that does not closely

resemble that of more deeply bound states, as is also ob-

served in Fig. 2. This is caused by the large spatial extent

( 100 bohr) of weakly bound wave functions, as illus-

The δ parameter in Eq. (4) is the phase difference

between the continuum channel wave functions and is

independent of the initial state of the photodissociated

molecules. It is thus readily amenable to a range of ap-

7

R

R

R

R

R

function is represented as an exponential with smoothly

varying amplitude and phase, and is a particularly use-

ful method of finding δ without using the full quantum

mechanical treatment.

The continuum wave function corresponding to the

partial wave J has the asymptotic behavior

  • 2 ,

(8)

0 u +

1 u

7 R R R R R function is represented as an exponential with smoothly varying amplitude
7 R R R R R function is represented as an exponential with smoothly varying amplitude
7 R R R R R function is represented as an exponential with smoothly varying amplitude
7 R R R R R function is represented as an exponential with smoothly varying amplitude
7 R R R R R function is represented as an exponential with smoothly varying amplitude
7 R R R R R function is represented as an exponential with smoothly varying amplitude
7 R R R R R function is represented as an exponential with smoothly varying amplitude
7 R R R R R function is represented as an exponential with smoothly varying amplitude
7 R R R R R function is represented as an exponential with smoothly varying amplitude
7 R R R R R function is represented as an exponential with smoothly varying amplitude
7 R R R R R function is represented as an exponential with smoothly varying amplitude
J i = 1
J i = 1
  • ψ J (R) sin kR + δ J

J i = 3
J i = 3
7 R R R R R function is represented as an exponential with smoothly varying amplitude
7 R R R R R function is represented as an exponential with smoothly varying amplitude
7 R R R R R function is represented as an exponential with smoothly varying amplitude
J i = 5
J i = 5
J i = 7
J i = 7
7 R R R R R function is represented as an exponential with smoothly varying amplitude
J i = 19
J i = 19
7 R R R R R function is represented as an exponential with smoothly varying amplitude
7 R R R R R function is represented as an exponential with smoothly varying amplitude
7 R R R R R function is represented as an exponential with smoothly varying amplitude

where k 2µε/ and µ is the reduced mass. An ana-

lytical expression for δ J is based on the WKB approxima-

tion where the wave function is assumed to have the form

ψ J (R) = e iS(R)/ . If only the lowest-order term in is

0 p(R)dR/ + π/4)

point and

p(R)

2µ(E V (R)) J(J + 1)/R 2 in terms of the molec-

ular potential V (R). The WKB approximation is most

applicable at higher energies and breaks down near the

turning point where p(R) 0. Based on the WKB ex-

pression for ψ(R) and Eq. (8), the asymptotic phase shift

is

δ WKB

J

=

R→∞

lim

R

  • 1

R 0

p(R)dR +

π

  • 4 kR +


2

.

(9)

  • kept in S(R), then ψ(R) sin(

7 R R R R R function is represented as an exponential with smoothly varying amplitude
7 R R R R R function is represented as an exponential with smoothly varying amplitude
7 R R R R R function is represented as an exponential with smoothly varying amplitude
7 R R R R R function is represented as an exponential with smoothly varying amplitude

where R 0

R

R

is the classical turning

7 R R R R R function is represented as an exponential with smoothly varying amplitude
  • A related approach to investigating the quantum-

7 R R R R R function is represented as an exponential with smoothly varying amplitude
7 R R R R R function is represented as an exponential with smoothly varying amplitude
7 R R R R R function is represented as an exponential with smoothly varying amplitude
7 R R R R R function is represented as an exponential with smoothly varying amplitude
7 R R R R R function is represented as an exponential with smoothly varying amplitude

quasiclassical crossover is to consider the classical rota-

tion of the molecule during photodissociation. We refer

to this method as the semiclassical approximation. Its

value is in the intuitive interpretation of the molecular

rotation angle during the bond breaking process and a

slightly faster computational convergence than the WKB

method. The angle of rotation γ between the initial

7 R R R R R function is represented as an exponential with smoothly varying amplitude

ε/h(MHz)

ε/h(MHz)

FIG. 4. Dependence of the amplitude-squared R parameter

from Eq. (4) on energy and on initial angular momentum

J i . The initial molecular states are 0

+

u

(0, J i , 0) (left column)

and 1 u (0, J i , 0) (right column), and P = 0. In each frame, the axial recoil limit is indicated by a horizontal line, and the highest rotational barrier in the continuum is shown by a dashed vertical line. For larger J i , the axial recoil limit is approached at higher energies, but in all cases the crossover from the ultracold to the quasiclassical regime occurs at the energy scale set by the barrier height. The initial states with J i = 3, 7, 19 exhibit shape resonance behavior.

molecular axis and the axis created by the scattered frag-

ments is γ J =

J(J + 1)/[p(R)R 2 ]dR. This angle
0

R

is connected to the anisotropy parameter β 2 by the rela-

tion β 2 = β AR P 2 (cos γ), where β AR takes on the limit-

ing values from the quasiclassical model [4–6] such that

β AR = {2, 1} for parallel and perpendicular photodis-

sociation transitions, respectively. This semiclassical ap-

proximation is more general than the quasiclassical model

which assumes that γ = 0.

The WKB method links the classical parameter γ to

the quantum mechanical phase δ J through γ = J /dJ

[20]. Further approximating the derivative by a difference

quotient yields the semiclassical approximation for the

phase shifts,

proximation techniques. We consider the WKB approxi-

mation [19, 20] and the semiclassical approximation [21],

and investigate their applicability to photodissociation

across a wide span of energies as well as their conver-

gence to the axial recoil limit.

The WKB approximation is a method of solving linear

differential equations with spatially varying coefficients.

It is applicable to approximating the solutions to the

time-independent Schr¨odinger equation, where the wave

δ J δ J = (J J) γ J + γ J .

2

(10)

The semiclassical approximation has been successfully

applied to diatomic molecule photodissociation at the en-

ergy of several wave numbers above threshold [21], where

a deviation from the axial recoil limit was observed, yield-

ing an agreement with quantum mechanical calculations

[22]. To summarize, the hierarchy of approximations,

8

J i = 1 cos δ
J i = 1
cos δ
J i = 3
J i = 3
J i = 5 J i = 7 ε/h(MHz) ε/h(MHz) cos δ
J i = 5
J i = 7
ε/h(MHz)
ε/h(MHz)
cos δ

FIG. 5. A comparison of the quantum mechanical, WKB, and

semiclassical methods for evaluating cos δ for a range of ini-

tial molecular angular momenta J i within the 0

+

u

electronic

manifold (here M i = P = 0).

The phase angle δ quanti-

fies interference between the two allowed dissociation channels and plays a key role in the observed photofragment angular distributions. Both approximations approach the quantum mechanical result at increasingly higher energies that are set by the rotational barrier heights (dashed vertical lines). All methods recover the axial recoil limit (horizontal lines) at high energies, but this convergence is slower for the δ parameter than for the R parameter in Fig. 4.

from the most to the least exact, is (i) quantum me-

chanical treatment, (ii) the WKB approximation, (iii) the

semiclassical model, and (iv) the axial recoil approxima-

tion (which is generally equivalent to the quasiclassical

model with exceptions discussed in Sec. V and Ref. [8]).

Figure 5 shows a comparison of the quantum mechan-

ical (Eq. (2)), WKB (Eq. (9)), and semiclassical (Eq.

(10)) approaches to calculating the δ parameter. This

phase angle is determined for the initial molecular states

J i = {1, 3, 5, 7} within the 0

+

u

electronic manifold, as-

suming photodissociation with M i = P = 0. We find

the applicability ranges of both approximation methods

to be similar, with the exception that the WKB approx-

imation is more accurate for very low J i . These ranges

are set by the barrier heights in the continuum, indicated

with dashed vertical lines. We also find that all methods

converge to the axial recoil limit cos δ = 1. However, this

convergence happens more slowly than for the R param-

eter in Fig. 4, and dominates the discrepancy between

the measured angular distributions and those expected

for axial recoil at energies beyond the barrier height, as

in Fig. 2 where the barrier height is only 10 MHz

but nonclassical behavior persists to 10 3 MHz [23].

Furthermore, only the quantum mechanical approach is

sensitive to shape resonances, for example one that is

visible in Fig. 5 at ε/h 250 MHz for J i = 7.

  • V. THE ROLE OF QUANTUM STATISTICS IN

PHOTODISSOCIATION

The equivalence of the quasiclassical approximation to

the axial recoil limit of the quantum mechanical model

holds for molecules in well-defined Ω i states under the

assumption that the photofragments are not identical

bosons or fermions. Section III E assumes that a molecule

with angular momentum J i

= 0 can dissociate into the

{J i 1, J i , J i +1} partial waves as allowed by E1 selection

rules.

Spin statistics can impose additional limitations on the

available continuum channels, as is the case for Sr 2 and

many other molecules. In the electronic ground state, J

is always even for Sr 2 composed of identical bosonic Sr

atoms and odd for Sr 2 composed of identical fermions.

In this work, we use bosonic 88 Sr and therefore J is

even. This restriction only affects Ω k = 0 electronic

states. Furthermore, in cases where Ω i = Ω k = 0 or

M i = M k = P = 0, the properties of the 3j symbols in

Eqs. (2,3) naturally force the continuum J to be only

even or odd, making the axial recoil approximation in-

sensitive to quantum statistics [24]. Here we extend Eq.

(3) to cases where quantum statistics must be considered,

and compare the results to the quasiclassical model (6).

In our experiment, this affects photodissociation from the

1 u states to the ground-state continuum, except in cases

where M i = P = 0.

First we assume that the photodissociation light po-

larization points along the quantization axis. The two

relevant cases are J = J i (applicable, for example, to

fermionic-Sr dimers dissociating from odd J i ) and J =

{J i 1, J i + 1} (applicable to bosonic-Sr dimers pho-

todissociating from odd J i as in our experiments). As

shown in the Appendix, we adapt the axial-recoil cross

section σ AR (θ, φ) to both quantum-statistics restricted

cases, and find the modified photodissociation cross sec-

tion, σ QS, (θ, φ). The result is analogous to the quasiclas-

sical cross section σ QC (θ, φ) in Eq. (6) but with the initial

J

angular probability density P i (θ, φ) = |D M i i (φ,

i

replaced by

θ, 0)| 2

P i, (θ, φ) = D M i ,1 (φ, θ, 0) σ i D M i ,1 (φ, θ, 0) 2 , (11)

J i

J i

where σ i p i (1) J i is the spectroscopic parity of the

initial state and p i is the parity with respect to space-

fixed inversion. For example, for 1 u initial states, p i = 1

for bosonic-Sr dimers and p i = 1 for fermionic-Sr dimers.

Next we treat the case where the photodissociation

light polarization is perpendicular to the quantization

axis. Again spin statistics enforces either J = J i or

J = {J i 1, J i + 1}. As detailed in the Appendix, we

adapt σ AR (θ, φ) to both cases and find the modified pho-

todissociation cross section

σ QS, (θ, φ)

(12)

J

cos 2 φ D M i ,1 (φ,

i

θ,

0)

+

σ i D

J

M i ,1 (φ,

i

θ, 0)

2

+

J

cos 2 θ sin 2 φ D M i ,1 (φ,

i

θ,

J

0) σ i D M i ,1 (φ,

i

θ, 0)

2

.

9

  • (a) quasiclassical

quantum

1 u (J i =1, M i =0, P=1)

1 u (J i =1, M i =1, P=1)

(a) quasiclassical quantum 1 ( J =1, M =0, P =1) 1 ( J =1, M
(a) quasiclassical quantum 1 ( J =1, M =0, P =1) 1 ( J =1, M
(a) quasiclassical quantum 1 ( J =1, M =0, P =1) 1 ( J =1, M
(a) quasiclassical quantum 1 ( J =1, M =0, P =1) 1 ( J =1, M
quantum (b) quasiclassical 1 ( J =3, M =2, P =0) 1 ( J =3, M
quantum (b) quasiclassical 1 ( J =3, M =2, P =0) 1 ( J =3, M
quantum (b) quasiclassical 1 ( J =3, M =2, P =0) 1 ( J =3, M
quantum (b) quasiclassical 1 ( J =3, M =2, P =0) 1 ( J =3, M

quantum

  • (b) quasiclassical

1 u (J i =3, M i =2, P=0)

1 u (J i =3, M i =1, P=0)

(c) 1 ( J =3, M =1, P =1) 1 ( J =3, M =0, P
(c) 1 ( J =3, M =1, P =1) 1 ( J =3, M =0, P
(c) 1 ( J =3, M =1, P =1) 1 ( J =3, M =0, P
(c) 1 ( J =3, M =1, P =1) 1 ( J =3, M =0, P

(c)

1 u (J i =3, M i =1, P=1)

1 u (J i =3, M i =0, P=1)

1 ( J =3, M =3, P =1) 1 ( J =3, M =2, P =1)
1 ( J =3, M =3, P =1) 1 ( J =3, M =2, P =1)
1 ( J =3, M =3, P =1) 1 ( J =3, M =2, P =1)
1 ( J =3, M =3, P =1) 1 ( J =3, M =2, P =1)

1 u (J i =3, M i =3, P=1)

1 u (J i =3, M i =2, P=1)

FIG. 6. Quasiclassical and quantum mechanical calculations of the photofragment angular distributions do not generally converge in the axial recoil limit if the photofragments are identical particles. Experimental measurements always agree with the quantum theory [17]. Here the high-energy angular distributions are calculated with the quasiclassical (6) and quantum mechanical (3) models for the 1 u initial states with (a) J i = 1, M i = {0, 1}, P = 1; (b) J i = 3, M i = {1, 2}, P = 0; and (c) J i = 3, M i = {0, 1, 2, 3}, P = 1.

This result is not analogous to the quasiclassical cross

section σ QC (θ, φ).

The photodissociation cross sections modified by spin

statistics are not correctly described by the quasiclassical

model (6), even in the axial recoil limit of large contin-

uum energies. This effect is observable in experiments

as a deviation of high-energy photodissociation images

from the quasiclassical model for certain initial molecu-

lar states and light polarizations [17].

Figure 6 illustrates 88 Sr 2 photodissociation pathways

where photofragment angular distributions in the axial

recoil limit (3) cannot be described by the quasiclassi-

cal model (6). In our experiment and in the figure, the

initial molecular states and laser polarizations that lead

to a non-quasiclassical axial recoil limit are (a) 1 u (J i =

1, M i = {0, 1}, P = 1); (b) 1 u (J i = 3, M i = {1, 2}, P =

0); and (c) 1 u (J i = 3, M i = {0, 1, 2, 3}, P = 1). The

case

considered in the top row of Fig. 6(a) results in a dis-

tribution that does not evolve with energy, since only a

single partial wave J = 2 is allowed in the continuum by

selection rules and hence the matrix elements in Eq. (5)

cancel for all energies [25]. Our experimental measure-

ments of angular distributions always agree with quan-

tum mechanical calculations [17]. For photodissociation

of molecules in analogous quantum states but composed

of identical fermionic isotopes we expect to observe differ-

ent distributions than in Fig. 6, and still different results,

that are well described by the quasiclassical model, are

expected for mixed dimers.

VI.

CONCLUSIONS

We report photodissociation with ultracold 88 Sr 2

molecules in isolated internal quantum states, including

different binding energies and angular momenta, where

we image and calculate the photofragment angular dis-

tributions as a function of the kinetic energy in the con-

tinuum, spanning from the ultracold to the quasiclassical

regime. At the higher energies that exceed the relevant

potential barriers, the distributions converge to a small

set of angular patterns that correspond to the axial recoil

limit where the molecule has no time to rotate during the

bond breaking process. In contrast, at the lower energies

the distributions exhibit strong variation with energy and

a dependence on the initial molecular state.

We utilize precise quantum state selection to ensure a

two-channel photodissociation outcome that can be de-

scribed by only two parameters: an amplitude that has

a weak dependence on the initial vibrational quantum

number and a phase that only depends on the contin-

uum wave functions. The amplitude converges to the

axial recoil limit significantly faster than the phase, with

a slower convergence for very weakly bound initial molec-

ular states. The WKB and semiclassical approximations

are shown to agree with the quantum mechanical model

at energies that exceed the barrier heights, and to cor-

rectly approach the axial recoil limit. Finally, we find

that in case of identical photofragments, the effects of

bosonic or fermionic statistics can persist into the high

energy regime, in which case the axial recoil limit dis-

agrees with the ubiquitous quasiclassical model.

The ability to access the crossover from the ultra-

cold to the quasiclassical regime of photodissociation

was enabled by quantum state control of the molecules,

making it possible to populate exclusively low-angular-

momentum states and thus access low partial waves in

the continuum that are strongly sensitive to quantum

effects. As more experiments begin to probe cold and ul-

tracold chemistry, including molecular photodissociation,

it is important to recognize the extent of the parameter

space where the processes are truly quantum mechanical.

Our work brings this insight into a long-debated issue

of the applicability of quasiclassical models to molecular

photodissociation, and elucidates which parameters limit

the convergence toward the high-energy limit.

ACKNOWLEDGMENTS

We acknowledge the ONR Grant No. N00014-17-1-

2246 and the NSF Grant No. PHY-1349725. R. M. and

I. M. also acknowledge the Polish National Science Center

10

Grant No. 2016/20/W/ST4/00314 and M. M. the NSF

IGERT Grant No. DGE-1069240.

Appendix: Axial recoil limit for identical photofragments

  • 1. Light polarization along the quantization axis

With the assumptions {i = 1, k = 0, M k = M i }, as

for Sr 2 photodissociation from the 1 u states to the ground

10 Grant No. 2016/20/W/ST4/00314 and M. M. the NSF IGERT Grant No. DGE-1069240. Appendix: Axial recoil

state continuum with light polarization along the quan-

tization axis (P = 0), the axial-recoil photodissociation

cross section (3) becomes

2 J k 1 J i J k σ(θ, φ) ∝ (−1) M i (2J
2
J k
1
J i
J k
σ(θ, φ) ∝ (−1) M i (2J k + 1)D
i 0 (φ, θ, 0)
.
(A.1)
M
−M i 0 M i J k 1 J i
0
−1
1
J k
a.
Partial waves restricted to J i
After restricting the allowed partial waves to J k = J i
and transforming the D-matrix as
J i (J i + 1)
J
J
J
D M i 0 (φ, θ, 0) = −
i
sin θ D M i ,−1 (φ, θ, 0) + D M i ,1 (φ, θ, 0) ,
i
i
(A.2)
2M i
Eq. (A.1) reads
Eq. (11).
J
J
σ(θ, φ)
∝ D M i ,−1 (φ, θ, 0) + D M i ,1 (φ, θ, 0) 2 sin θ 2 .
i
i
b.
Partial waves restricted to J i ± 1
(A.3)
After restricting the partial waves to J k = J i ± 1, the
This cross section has the form of Eq.
(6) with β 2 = −1
cross section in Eq. (A.1) can be manipulated by tak-
(as expected for this ∆Ω = 1 transition), with the initial
ing the sum over all partial waves and subtracting the
angular probability density replaced by the expression in
forbidden contributions,
J k
1
J i
J k
σ(θ, φ) ∝
(−1) M i (2J k + 1)D
i 0 (φ, θ, 0)
+
(A.4)
M
−M i 0 M i J k 1 J i
0
−1
1
J k ={J i −1,J i ,J i +1}
2
J
J i
1
J i
− (−1) M i (2J i + 1)D M i 0 (φ, θ,
i
0)
=
−M i 0 M i J i 1 J i
0
−1
1
1
J
J
J
= D 0,−1 (φ, θ, 0)D M i ,1 (φ, θ, 0) + (−1) M i (2J i + 1) D M i ,−1 (φ, θ, 0) + D M i ,1 (φ, θ, 0) sin θ
i
i
i
× J i (J i + 1)
2
J i
1
J i
=
2M i
−M i 0 M i J i 1 J i
0
−1
1
2
1
1
J
J
J
= −
sin θD M i ,1 (φ, θ, 0) +
i
2 √ 2 sin θ D M i ,−1 (φ, θ, 0) + D M i ,1 (φ, θ, 0)
i
i
√ 2
1
2
J
J
=
D M i ,1 (φ, θ, 0) − D M i ,−1 (φ, θ, 0)
i
i
sin 2 θ.
8

11

The second step of Eq. (A.4) uses Eq.

(A.2) as well as

the summation (Clebsch-Gordan series)

11 The second step of Eq. (A.4) uses Eq. (A.2) as well as the summation (Clebsch-Gordan

(1) M k + k (2J k + 1)D

J k

= D M k k (φ, θ, 0)

J k

J k

= D

J i

  • M i i

1

  • D P Q .

J k 1 J i J k 1 J i J k k Ω k (φ,
J k
1
J i
J k
1
J i
J k
k Ω k (φ, θ, 0)
(A.5)
M
−M k P M i −Ω k Q Ω
i =
J k
1
J i
J k
1
J i
−M k P M i −Ω k Q Ω
i =
  • 2. Light polarization normal to the quantization axis

With the assumptions {i = 1, k = 0, M k = M i ±1},

as for Sr 2 photodissociation from the 1 u states to the
as
for
Sr 2
photodissociation from the 1 u states to the

ground state continuum with light polarization normal

to the quantization axis (P = ±1), the axial-recoil cross

section (3) becomes

σ(θ, φ) (1) M k (2J k + 1)D

J k P

1 2 J k J i J k k 0 (φ, θ, 0) . (A.6) M
1
2
J k
J i
J k
k 0 (φ, θ, 0)
.
(A.6)
M
−M k
P
M i
  • a. Partial waves restricted to J i

After restricting the partial waves to J k = J i , summing

over P, and evaluating the 3j symbols, the cross section

in Eq. (A.6) becomes

σ(θ, φ) ∝(2J i + 1) J i 1 J i 0 −1 1
σ(θ, φ) ∝(2J i + 1) J i 1 J i
0
−1
1
 

(A.7)

 

2

  • 1 (A.8)

2

J

i

cos θ

D M i ,1 (φ, θ, 0) ,

  • 1 (A.9)

2

J

i

cos θ

D M i ,1 (φ, θ, 0)

× D M i +1,0 (φ, θ, 0) (J i M i )(J i + M i + 1) D M i 1,0 (φ, θ, 0) (J i + M i )(J i M i + 1) .

J i

J i

11 The second step of Eq. (A.4) uses Eq. (A.2) as well as the summation (Clebsch-Gordan

We use the recursion formulas [26]

J i (J i + 1) M i + 1) 1 + cos θ J
J i (J i + 1) M i + 1) 1 + cos θ
J
D M i +1,0
J
i
(φ,
θ, 0)e iφ =
i
θ, 0)
D M i ,−1 (φ,
(J i − M i )(J i +
2
J i (J i + 1) M i + 1) 1 + cos θ
J
D M i −1,0
J
i
(φ,
θ, 0)e −iφ =
i
θ, 0) −
D M i ,1 (φ,
(J i + M i )(J i −
2
11 The second step of Eq. (A.4) uses Eq. (A.2) as well as the summation (Clebsch-Gordan

to transform Eq. (A.7) into

12

J i J ∝ cos 2 φ D M i ,1 (φ, θ, i J i
J
i
J
∝ cos 2 φ D M i ,1 (φ, θ,
i
J i
b.
Partial waves restricted to J i ± 1
With the partial waves limited to J k
=
J i ± 1,
the
cross section in Eq. (A.6) can again be manipulated by
J k
σ(θ, φ) ∝ (−1) M k (2J k + 1)D
M
J k P
J i
After applying Eqs. (A.2) and (A.8,A.9) to the first and
J i
1
1
J i

σ(θ, φ) D M i ,1 (φ, θ, 0) × (cos φ + i cos θ sin φ) D M i ,1 (φ, θ, 0) × (cos φ i cos θ sin φ) 2

J

i

2

.

(A.10)

0) D M i ,1 (φ, θ, 0) 2 + cos 2 θ sin 2 φ D M i ,1 (φ, θ, 0) + D M i ,1 (φ, θ, 0)

J i

J i

12 J i J ∝ cos 2 φ D M i ,1 (φ, θ, i J

taking the sum over all partial waves and subtracting the

forbidden contributions,

k 0 (φ, θ, 0)

M k P M i J k 1 J i

J k

1

J i

0

−1 1
−1
1

1

2

.

(A.11)

(1) M k (2J i + 1)D M k 0 (φ, θ, 0)

M k P M i J i 1 J i

J i

1

J i

0

1

12 J i J ∝ cos 2 φ D M i ,1 (φ, θ, i J

second term on the right-hand side of Eq. (A.11), respec-

tively, we obtain the cross section

σ(θ, φ) D M i ,1 (φ, θ, 0) D 1,1 (φ, θ, 0) + D 1,1 (φ, θ, 0) +

2

2

=

1

J

D M i ,1 (φ, θ, 0) × (cos φ + i cos θ sin φ)

i

  • 2 1 D M i ,1 (φ, θ, 0) × (cos φ i cos θ sin φ)

= D M i ,1 (φ, θ, 0) × (cos φ + i cos θ sin φ) + D M i ,1 (φ, θ, 0) × (cos φ i cos θ sin φ) 2

J i

J i

(A.12)

J i

cos 2 φ D M i ,1 (φ, θ, 0) +

D M i ,1 (φ, θ, 0) 2 + cos 2 θ sin 2 φ D M i ,1 (φ, θ, 0) D M i ,1 (φ, θ, 0)

J i

J i

J i

2

.

12 J i J ∝ cos 2 φ D M i ,1 (φ, θ, i J

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